Low-temperature Reverse Water-Gas Shift Reaction Using SILP Ru Catalysts under Continuous-flow Conditions

Ionic liquids (ILs) are considered to be potential material devices for CO 2 capturing and conversion to energyadducts. They form a cage (confined-space) around the catalyst providing an ionic nano-container environment which serves as physical-chemical barrier that selectively controls the diffusion of reactants, intermediates, and products to the catalytic active sites via their hydrophobicity and contact ion pairs. Hence, the electronic properties of the catalysts in ILs can be tuned by the proper choice of the IL-cations and anions that strongly influence the residence time/diffusion of the reactants, intermediates, and products in the nano-environment. On the other hand, ILs provide driving force towards photocatalytic redox process to increase the CO 2 photoreduction. By combining ILs with the semiconductor, unique solid semiconductor-liquid commodities are generated that can lower the CO 2 activation energy barrier by modulating the electronic properties of the semiconductor surface. This mini-review provides a brief overview of the recent advances in IL assisted thermal conversion of CO 2 to hydrocarbons, formic acid, methanol, dimethyl carbonate, and cyclic carbonates as well as its photo-conversion to solar fuels.

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“…When they replaced Ru catalyst to [Ru-(CO) 3 Cl 3 ] 2 , about 1500 TONs were achieved at 210 °C. [30]…”

Section: Co 2 Hydrogenation To Hydrocarbons In Bare Ilsmentioning

confidence: 99%

“…The authors believed that SiO 2 support lowered the activation energy of the protonation reaction to enhance RWGS process. When they replaced Ru catalyst to [Ru(CO) 3 Cl 3 ] 2 , about 1500 TONs were achieved at 210 °C [30] …”

Section: Thermal Co2 Activation In Ilsmentioning

confidence: 99%

Thermo‐ and Photocatalytic Activation of CO₂ in Ionic Liquids Nanodomains

Qadir

Dupont

2023

Angewandte Chemie

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“…These and other special characteristics have rendered ILs as interesting working fluids for a wide range of technical applications in both research and industry [1][2][3][4][5]. For example, ILs can be used as electrolytes [1,6], media for heat transfer and energy storage [7,8] or for gas separation [9,10] as well as solvents for catalysis in Supported Ionic Liquid Phase (SILP) systems [11]. SILP materials involve homogeneous catalysts in the form of metal complexes dispersed in thin IL films coated on solid supports [12][13][14][15].…”

Section: Introductionmentioning

confidence: 99%

Influence of Molecular Hydrogen on Bulk and Interfacial Properties of Three Imidazolium-Based Ionic Liquids by Experiments and Molecular Dynamics Simulations

Zhai,

Hantal,

Cherian

et al. 2024

Preprint

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Despite the presence of molecular hydrogen (H2) in various technical applications involving ionic liquids (ILs), its effect on the bulk and interfacial properties of ILs is poorly understood. The present study investigates the influence of dissolved H2 on the viscosity, surface tension, and phase composition of three imidazolium-based ILs by experiments and Molecular Dynamics (MD) simulations between (303 and 393) K from (0.1 to 31) MPa. The surface light scattering and pendant-drop experiments showed for all three ILs that the saturated liquid viscosity does not significantly change with increasing H2 pressure, while the surface tension decreases about 5% at 8 MPa. The MD simulations could be used to clarify microscopic origins for the behavior of the macroscopic properties. They revealed not only a compensation of compression and solvation effects due to hydrostatic pressure and dissolved H2 on the viscosity, but also a weak enrichment of H2 at the IL-gas interfaces.

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“…In addition, catalytic activity remained stable even after 30 h when the catalyst was used in a fixed-bed flow reactor system. 20 In this study, we applied the SILP catalyst technology to the hydroformylation of propene with CO 2 catalyzed by Ru complexes derived from Ru 3 (CO) 12 and imidazolium chlorides (eq 1). Surprisingly, the SILP catalyst not only enabled the use of CO 2 as a reactant in such a key reaction in the chemical industry, but it also facilitated the replacement of the batch reaction process with a continuous flow reaction process.…”

Section: ■ Introductionmentioning

confidence: 99%

“…The SILP catalyst could be reused 20 times, and the total turnover number per Ru atom reached 3600. In addition, catalytic activity remained stable even after 30 h when the catalyst was used in a fixed-bed flow reactor system …”

Section: Introductionmentioning

confidence: 99%

Continuous Gas-Phase Hydroformylation of Propene with CO₂ Using SILP Catalysts

Hatanaka

Yasuda

Uchiage

et al. 2021

ACS Sustainable Chem. Eng.

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Hydroformylation is an important process for the synthesis of aldehydes and alcohols in the chemical industry. Although this process uses toxic CO as one of the reactants, some types of Ru complex catalysts have been known to replace CO with CO2 as a reactant in hydroformylation. Herein, we report the continuous hydroformylation of propene with CO2, heterogeneously catalyzed by supported Ru complexes on silica using ionic liquids [i.e., supported ionic liquid-phase (SILP) catalysts] in a flow reactor. When the reaction was carried out at 170 °C, 8.6 MPa, and gas hourly space velocity (GHSV) of 1.13 × 103 h–1 using the SILP catalyst prepared from Ru3(CO)12, 1-ethyl-3-methylimidazolium chloride, and silica, the conversion of propene was 81.6% and the selectivity of hydroformylation was 66.1%. Kinetic analysis showed that the reaction rates of CO formation and hydroformylation were near-identical at 170 °C, indicating that the CO formed by the reverse water–gas shift reaction was readily used for the subsequent hydroformylation reaction. ESI-MS analysis of the ionic liquid phase showed the formation of trinuclear and mononuclear Ru complexes, and a plausible reaction mechanism was proposed based on these findings.

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Low-temperature Reverse Water-Gas Shift Reaction Using SILP Ru Catalysts under Continuous-flow Conditions

Cited by 7 publications

References 12 publications

Thermo‐ and Photocatalytic Activation of CO₂ in Ionic Liquids Nanodomains

Thermo‐ and Photocatalytic Activation of CO₂ in Ionic Liquids Nanodomains

Influence of Molecular Hydrogen on Bulk and Interfacial Properties of Three Imidazolium-Based Ionic Liquids by Experiments and Molecular Dynamics Simulations

Continuous Gas-Phase Hydroformylation of Propene with CO₂ Using SILP Catalysts

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Low-temperature Reverse Water-Gas Shift Reaction Using SILP Ru Catalysts under Continuous-flow Conditions

Cited by 7 publications

References 12 publications

Thermo‐ and Photocatalytic Activation of CO2 in Ionic Liquids Nanodomains

Thermo‐ and Photocatalytic Activation of CO2 in Ionic Liquids Nanodomains

Influence of Molecular Hydrogen on Bulk and Interfacial Properties of Three Imidazolium-Based Ionic Liquids by Experiments and Molecular Dynamics Simulations

Continuous Gas-Phase Hydroformylation of Propene with CO2 Using SILP Catalysts

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Product

Resources

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Thermo‐ and Photocatalytic Activation of CO₂ in Ionic Liquids Nanodomains

Thermo‐ and Photocatalytic Activation of CO₂ in Ionic Liquids Nanodomains

Continuous Gas-Phase Hydroformylation of Propene with CO₂ Using SILP Catalysts